Electronic Couplings versus Thermal Fluctuations in the Internal Conversion of Perylene Diimides: The Battle to Localize the Exciton
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Le résumé fourni par la source
Energy transfer processes among units of light-harvesting homo-oligomers impact the efficiency of these materials as components in organic optoelectronic devices such as solar cells. Perylene diimide (PDI), a prototypical dye, features exceptional light absorption and highly tunable optical and electronic properties. These properties can be modulated by varying the number of PDI units and linkers between them. Herein, atomistic nonadiabatic excited state molecular dynamics is used to explore the energy transfer during the internal conversion of acetylene and diacetylene bridged dimeric and trimeric PDIs. Our simulations reveal a significant impact of the bridge type on the transient exciton localization/delocalization between units of PDI dimers. After electronic relaxation, larger exciton delocalization occurs in the PDI dimer connected by the diacetylene bridge with respect to the one connected by the shorter acetylene bridge. These changes can be rationalized by the Frenkel exciton model. We outline a technique for deriving parameters for this model using inputs provided by nonadiabatic dynamics simulations. Frenkel exciton description reveals an interplay between the relative strengths of the diagonal and off-diagonal disorders. Moreover, atomistic simulations and the Frenkel exciton model of the PDI trimer systems corroborate in detail the localization properties of the exciton on the molecular units during the internal conversion to the lowest-energy excited state when the units become effectively decoupled. Overall, atomistic nonadiabatic simulations in combination with the Frenkel exciton model can serve as a predictive framework for analyzing and predicting desired exciton traps in PDI-based oligomers designed for organic electronics and photonic devices.
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Le contrôle bibliographique ouvert
DOI retrouvé dans Crossref DOI retrouvé ; titre concordant.
- Titre Crossref
- Electronic Couplings versus Thermal Fluctuations in the Internal Conversion of Perylene Diimides: The Battle to Localize the Exciton
- Date Crossref
- 10/07/2024
- Éditeur
- American Chemical Society (ACS)
- Type
- journal-article
Ce recoupement confirme des métadonnées liées au DOI. Il ne confirme ni la méthode ni les conclusions de l’étude, et il ne compte pas comme une seconde source scientifique indépendante.
Où se fait cette recherche
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National University of Quilmes pays non établi dans la noticeUniversité ou école supérieure
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Consejo Nacional de Investigaciones Científicas y Técnicas pays non établi dans la noticeOrganisme public
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University of California Department of Chemistry and Physics and Astronomy pays non établi dans la noticeUniversité ou école supérieure
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Boston University Division of Materials Science and Engineering pays non établi dans la noticeUniversité ou école supérieure
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Los Alamos National Laboratory and Center for Integrated Nanotechnologies (CINT) pays non établi dans la noticeStructure de recherche
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Center for Integrated Nanotechnologies pays non établi dans la noticeStructure de recherche
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Departamento de Ciencia y Tecnologia pays non établi dans la noticeInstitution
National University of Quilmes, Consejo Nacional de Investigaciones Científicas y Técnicas et Department of Chemistry and Physics and Astronomy — University of California, avec 4 autres affiliations.
Une affiliation ne permet pas de déduire la nationalité d’un auteur.